Molecular simulation of thermosetting polymer hardening: reactive events enabled by controlled topology transfer

Abstract: We present a quantum mechanical / molecular mechanics (QM/MM) to tackle chemical reactions with substantial molecular reorganization. For this, molecular dynamics simulations with smoothly switched interaction models are used to suggest suitable product states, whilst a Monte Carlo algorithm is employed to assess the reaction likeliness subject to energetic feasibility. As a demonstrator, we study the cross-linking of bisphenol F diglycidyl ether (BFDGE) and 4,6-diethyl-2-methylbenzene-1,3-diamine (DETDA). The modeling of epoxy curing was supplemented by Differential Scanning Calorimetry (DSC) measurements, which confirms the degrees of cross-linking as a function of curing temperature. Likewise, the heat of formation and the mechanical properties of the resulting thermosetting polymer are found to be in good agreement with previous experiments.